The role of Mo in the passivation of stainless steels was investigated using ac impedance spectroscopy. Six steels were examined : two ferritic (Fe-20Cr) alloys containing 0 and 1% Mo and four austenitic (Fe-20Cr-25Ni) alloys containing 0, 1, 2, and 4.5% Mo. The experiments were performed in 1 M HCl and, in some cases, 0.5 M H2SO4, 1 M HCl + 3 M NaCl, and 4 M HCl. Quasi-steady-state polarization curves were obtained and the impedance was measured at potentials in the active region and through the active-to-passive transition. The impedance spectra exhibited up to four arcs with well-resolved time constants. Equivalent circuit parameters were evaluated in each case to examine the effect of Mo on the dissolution of the alloys. Mo appears to influence virtually all of the principal reactions involved in the dissolution, intermediate formation, and passivation of stainless steels. Its effect is complex and extends beyond a single reaction step in the mechanism for the dissolution and passivation of these alloys.